The invention relates to a stratified phase-separated composite, a method of manufacturing such a composite and photo-chemically reactive compositions for use in such a method.
In Science vol.283 (1999) page 1903, Kumar et al (see also U.S. Pat. No. 5,949, 508) disclose a phase-separated composite and a method of manufacturing such. The known composite is manufactured by providing, between a pair of opposed substrates, a layer of a photo-polymerizable monomer (prepolymer) dissolved in an organic liquid, in particular a liquid crystal. The organic liquid and monomer are selected such that the liquid is poorly miscible with the photo-polymerized monomer. If so selected, phase-separation of the liquid and the photo-polymer takes place during photo-polymerization, a process known in the art as polymerization-induced phase separation (PIPS). In the composite of Kumar et al. the organic liquid is furthermore adapted to absorb the UV light used for photo-polymerizing the monomer. Therefore, according to Kumar et al, upon subjecting the layer to UV light, a light intensity gradient is set up in the layer in directions normal to the layer, the highest intensity occurring at the side layer facing the UV light source. Since the rate at which photo-polymerization takes place scales with the intensity of UV light, photo-polymerization and therefore phase-separation preferentially takes place at the side of the layer facing the light source. As a result the phase-separation takes place in a stratified manner, producing composite comprising a predominantly polymeric layer formed at the UV light source side and a predominantly liquid layer at the side facing away from the UV light source.
The range of liquid crystals which can be suitably used to form a stratified-phase-separated composite is limited to those which absorb the radiation used to bring about phase-separation. However, for many applications, the use of other liquid crystals would be desirable. In particular, liquid crystal used by Kumar, E7, a cyanobiphenyl LC is not suitable for use in AMLCD. A further disadvantage of the known composite may be that the phase-separation is not perfect. In particular, small amounts of LC material are still present in the polymeric layer. For many applications such inclusions of LC material may be undesirable. For example, the liquid crystal inclusions may give rise to spurious switching effects and if LC inclusions during the useful lifetime migrate to and merge with the liquid layer the properties, such as retardation or orientation, may be affected.
It is an object of the invention, inter alia, to provide a stratified phase-separated composite which does not have these drawbacks. In particular, it is an object to extend the range of stratified-phase-separated composites by extending the range of fluids suitable for use in a such a composite. A further object may be to provide a composite which may have an improved phase-separation.
In accordance with the invention, these objectives are achieved by a stratified phase-separated composite a stratified phase-separated composite comprising a photo-polymeric layer and a liquid layer, the composite being obtainable by photo-polymerizing a layer of a photo-polymerizable stratified-phase-separable composition, the composition comprising:
a photo-polymerizable monomer;
a photo-polymerization dye which, during photo-polymerization, selectively accumulates in the photo-polymeric layer being formed; and
a liquid.
The stratified-phase-separated composite in accordance with the invention is, like the known composite, obtainable by photo-polymerization induced phase-separation. It differs from the known composite in that the stratified-phase-separated composite in accordance with the invention comprises a photo-polymerization dye which is selectively accumulated in the polymeric layer, where in the context of the invention, the term xe2x80x9cphoto-polymerization dyexe2x80x9d refers to a compound which is adapted to at least partially absorb the actinic radiation used for photo-polymerizing the monomeric material.
Since the required intensity gradient is provided by the photo-reactive photo-polymerization dye, the liquid (crystal) may but need not be light-absorbing. The range of liquids which can be suitably used in the composite in accordance with the invention is thus significantly increased. Also, having the photo-polymerization dye as a separate component gives more flexibility in selecting the desired light intensity gradient. After all, in case the absorption is predominantly determined by the liquid crystal, as is the case in the prior art composite, selecting the desired thickness of the liquid layer in the composite already fixes the light intensity gradient and thus the stratification process.
The addition of a dye which selectively accumulates in the polymeric layer may improve the phase-separation. In particular, the improved phase separation may take the form of a reduction of the amount of liquid enclosed in the polymeric layer and/or an improvement in the uniformity of the interface between the liquid and polymeric layer. Although not wishing to be bound by any theory it is noted that adding a photo-polymerization dye (as a component separate from the liquid) changes the absorption of the stratified-phase-separable layer and thus the intensity gradient set up in that layer both at the beginning and during photo-polymerization compared to the known composite in which the liquid serves as the absorbing material. In particular, adding such a dye renders the layer significantly more absorptive and/or the transition from high to low intensity significantly more steep. Moreover, since the dye selectively accumulates in the polymeric layer being formed an intensity gradient is obtained which is different from the gradient obtained using a dye which is either uniformly distributed in the phase-separable layer or a dye which selectively accumulates in the liquid layer such as the light absorbing liquid crystal used by Kumar.
Furthermore, if the composite is used in a device in which the liquid layer is an active layer, such as an LC device, it may be of disadvantage that the photo-polymerization dye is present in such an active layer. After all, generally, the dye serves a purpose during manufacture of the composite but after that, so during use or further manufacture, it has served this purpose and there isxe2x80x94for this purposexe2x80x94no longer a need for it to be present. Instead during use or further manufacture the dye may in fact have an adverse effect. For example, if a UV photo-polymerization dye is used the liquid may photo-degrade more easily over time. The dye may also influence the electro-optical properties of the liquid such as in particular its dielectric constant and birefringence. By selectively accumulating the dye in the polymeric layer, these adverse effects are avoided. In addition, the amount of dye can be selected freely without having to consider its effect on the liquid layer.
In a broad sense, the invention relates to any stratified-phase-separated composite which comprises a photo-polymerization dye as a component separate from the liquid as long as the dye, at least partially, absorbs the radiation used to photo-polymerize the monomers. However, in general the dyes have a tendency to selectively accumulate in the liquid layer instead of in the polymeric layer.
Generally, dyes which selectively accumulate in the polymeric layer may be found by selecting a dye which dissolves better in the (partially polymerized) monomer than in the liquid. A difference in solubility can be obtained by combining a liquid with a monomer or (partially) polymerized forms thereof having a polarity substantially different from the liquid. For example if the liquid is an apolar liquid the polymer may be polar or rendered polar by functionalizing with polar substituents or even ionic groups. If the dye is selected to be polar or similarly rendered polar selective accumulation in the polymeric layer is obtained.
A further means to promote selective accumulation in the polymeric layer, comprises providing means to chemically bond the dye to (partially polymerized) monomers. Accordingly, in a preferred embodiment of the stratified-phase-separated composite in accordance with the invention, the photo-polymerization dye is a photo-chemically reactive dye which, during photo-polymerization, is capable of photo-chemically bonding to photo-polymerizable or photo-polymerized monomers.
In photo-chemically bonding the dye to the monomers or polymerized monomers, the (polymerized) monomers force the dye into the polymeric layer being formed thus obtaining selective accumulation in the polymeric layer. By using such a photo-chemically reactive dye, any photo-polymerization dye, in particular any conventional dye, may be rendered capable of selectively accumulating in the polymeric layer. All that needs to be done is to provide the dye with a photo-reactive group which, during polymerization, is capable of photo-chemically bonding to photo-polymerizable or photo-polymerized monomers. Since the dye is chemically bonded to the monomer, the risk of the photo-polymerization dye being released into the liquid layer during further use of the composite is also reduced. The dye is effectively encapsulated in the polymeric layer.
A convenient choice of photo-reactive dye is one wherein a photo-polymerization dye is functionalized with a photo-polymerizable group.
Therefore, in a preferred embodiment the photo-chemically reactive dye is a photo-polymerizable dye co-polymerizable with the photo-polymerizable monomer.
By selecting the photo-polymerizable dye to be co-polymerizable with the monomer, phase-separation of different polymeric components within the polymeric layer is avoided. Moreover, if the dye and the monomer are functionalized with the same photo-polymerizable group, the photo-reaction of the dye and the monomer the reaction rates and other relevant photo-reaction parameters are very similar resulting in a homogeneous and controlled photo-reaction.
In order to reduce the number of distinct components, in a particular embodiment of the composite in accordance with the invention, the photo-polymerizable dye and the photo-polymerizable monomer are one and the same monomer.
In order to shorten the time of photo-polymerization, it may be of advantage to reduce the absorbance of the stratified-phase-separable layer during photo-polymerization. To achieve this, in a preferred embodiment of the composite in accordance with the invention is characterized in that the photo-polymerization dye is a photo-bleachable dye.
Photo-bleachable dyes are known as such. In a particularly preferred embodiment the photo-polymerization dye is functionalized with a photo-polymerizable group and a photo-bleachable group. A photo-bleachable photo-polymerization dye is a dye of which the absorbance decreases as a function of photo-polymerization-inducing radiation dose received. A first class of photo-bleachable dye has a chromophore which is photo-cleavable, the photo-cleavage products absorbing not or at least to a smaller extent the radiation bringing about photo-polymerization. A second class is formed by the class of photo-chromic dyes which possess on the one hand a state which absorbs the radiation which brings about photo-polymerization and on the other hand a state which does not. Photo-chromic dyes are well known. Another class of photo-bleachable dyes is the class of photo-isomerizable dyes having a first isomer which does absorb radiation bringing about photo-polymerization and a second isomer which does not do so, the first isomer being convertible into the second upon subjecting the first isomer to radiation which brings about photo-polymerization. An example of such a dye is a dye functionalized with a group comprising an isomerizable double bond such as a stilbene group. Another class consists of photo-oxidizable photo-polymerization dyes.
In a further aspect, the invention relates to a stratified phase-separated composite in accordance with the invention wherein the stratified-phase-separable composition is a photo-crosslinkable stratified-phase-separable composition.
The use of composition which is photo-crosslinkable may improve phase-separation, in particular in the sense of reducing the number of liquid molecules present (present in dissolved and/or dispersed form) in the polymeric layer and/or improving the uniformity of the liquid layer-polymeric layer interface. Furthermore, in case the liquid layer is a liquid crystal layer, the use of photo-crosslinkable monomer may render the composite combinable with an extended range of alignment layers in order to achieve an oriented liquid crystal layer.
A photo-crosslinkable composition produces upon irradiation a crosslinked polymer. A crosslinked polymer, also referred to as a network polymer, has crosslinks which link polymer chains to each other to form a three-dimensional network. Examples of photo-crosslinkable compositions are well known in the art. A typical example of a photo-crosslinkable monomer composition comprises a monomer, which if photo-polymerized neat forms a linear polymer chain, and a photo-crosslinking agent. To provide the light intensity gradient required to bring about stratification, the photo-crosslinkable stratified-phase-separable composition comprises a photo-polymerization dye. Since the measure of rendering the composition photo-crosslinkable may be taken in conjunction with or separate from the provision of a selectively accumulating dye, the photo-polymerization dye may also be the liquid or a component of the liquid. Preferably however a photo-polymerization dye which selectively accumulates in the polymeric layer is used. Further advantages of cross-linked polymers is improved temperature and mechanical resistance and resistance to chemicals such as solvents which is convenient if the polymeric layer is to serve as a substrate for wet depositing further layers.
In another aspect, the invention seeks to enlarge the class of photo-polymerized phase-separated composites.
This objective is met by a stratified phase-separated composite comprising a photo-polymeric layer and a liquid layer, the composite being obtainable by photo-polymerizing a layer of a photo-polymerizable stratified-phase-separable composition, the composition comprising:
a photo-polymerizable monomer;
a photo-polymerization dye; and
a liquid,
wherein the photo-polymerizable monomer is an acrylate or a methacrylate monomer.
Photo-polymerizable (meth)acrylates are suitable monomers to obtain photo-polymerized phase-separated composites. By employing (meth)acrylates, phase-separated composites may be obtained which have excellent phase-separation, that is the number of liquid molecules present (present in dissolved and/or dispersed form) in the polymeric layer may be very low and/or the interface of the liquid layer and the polymeric layer is very uniform. In particular, the uniformity may be such that protrusions which extend from the polymeric layer across the entire thickness of the liquid layer are absent. The use of (meth)acrylate monomers is an independent aspect of the invention as (meth)acrylate monomers may be used in conjunction with or separate from the use of a photo-crosslinkable monomer and/or a photo-reactive photo-polymerization dye. Preferably, however, a photo-reactive (meth)acrylate dye and/or a photo-crosslinkable (meth)acrylate is used. In addition, the use of (meth)acrylates may widen the choice of alignment layers which may be combined with the composites in accordance with the invention.
Suitable other photo-polymerizable monomers and/or photo-polymerizable dyes include a monomer of a thiol-ene system, an epoxide, a vinylene, a vinylether, an oxetane or a cinnamate
Particular suitable are photo-polymerizable monomers and/or dyes having one photo-polymerizable group which form main-chain and/or side-polymers, such as mono-(meth)acrylates, mono-epoxides, mono-vinylethers, mono-vinylenes, and dithiol thiol-ene systems. A cinnamate monomer which polymerizes via a step addition reaction requires two cinnamate groups to form a linear polymer chain. To obtain crosslinked polymers monomers comprising two or more photo-polymerizable groups, such as di(meth)acrylates, di-vinlyethers, di-oxetanes, di-vinylenes, di-epoxides, or thiol-ene systems comprising trithiol, a tri-ene, or di-enes provided with a mercapto group or ene-functionalized dithiols or higher homologues of such monomers, all of which are known in the art per se, may be used. Cross-linked cinnamates require monomers carrying at least three cinnamate groups. Particularly preferred are combinations of monomers having one photo-polymerizable group and monomers having two or more photo-polymerizable groups as they allow the degree of cross-linking to be freely selected.
The stratified-phase-separable material may comprise just one type of monomer to produce a homopolymer but generally it will contain more than one type to obtain copolymers, terpolymers or higher. The monomer may itself be a polymer also referred to as a prepolymer which is further polymerized. Different non-co-polymerizable monomers may also be used to obtain a polymer blend which may or may not be phase-separated.
Combinations of liquid crystal and monomers which may be suitable candidates for use in the stratified-phase-separable compositions in accordance with the invention are those used to manufacture polymer dispersed liquid crystals.
The photo-polymerization to be performed in order to obtain the stratified-phase-separated composite is as such conventional. It is not essential, yet convenient to include a photo-initiator in the stratified-phase-separable material to initiate the photo-polymerization. Conventional photo-initiators are suitable for this purpose. The photo-polymerization is performed using actinic radiation such as e-beam or ion beam radiation or electromagnetic radiation such x-ray or gamma-ray radiation. Generally, it is preferable to use less energetic radiation which is still sufficiently energetic to break or form covalent bonds, such as UV and visible light. Since many optical devices, such as displays, are to be active in the visible range of the spectrum radiation UV radiation is preferred, in particular UV light above 300 nm as glass becomes absorbing below 300 nm. The photo-polymerization may be performed as a flood exposure or in accordance with a desired pattern, for example using a mask or a combination thereof.
There is no limit on the type of liquid which may be used for the composite in accordance with the invention other than it should be able to form a liquid layer by means of stratified phase-separation. Examples include inorganic liquids such as water or water-based liquids and organic liquids such as solvents. The liquid may in particular be an electro-optical liquid, such as a liquid for use in an electrophoretic display or a liquid crystal display.
In a particularly suitable embodiment, the liquid is a liquid crystal.
Suitable liquid crystals include those capable of forming a planar, a homeotropic, a twisted or splay orientation. The orientation can also be uniaxial or biaxial. Any LC phase may be suitably used, such as nematic, twisted nematic, cholesteric, discotic, smectic A and C, ferroelectric, flexoelectric and the like. The liquid crystal layer may be partitioned into a number of distinct domains, each domain having a different anisotropic orientation such as a sub-pixel domain. In particular, the difference in orientation may be limited to a difference in the orientation of the director(s) while the type of anisotropy is the same.
The liquid may also be a polymerizable or polymerized liquid. The latter, being a solid, is of particular advantage in applications where the fluid nature of the liquid is of no relevance for the function to be achieved.
The thickness of the liquid layer will depend on the particular application sought but generally will vary from 0.1 xcexcm to 1 mm. In case the liquid layer is a liquid crystal layer the thickness will typically be 0.5 xcexcm to 10 xcexcm or more particular, 1 xcexcm to 5 xcexcm. The thickness of the polymeric layer will depend on its function in the composite. If the polymeric layer as such does not have to provide the necessary protection and/or ruggedness, resistance to tear and other mechanical forces, but has to be capable of providing a substrate surface for the provision of subsequent layers such as layers which do provide the necessary ruggedness and/or mechanical integrity the polymeric layer can be relatively thin, typically 0.1 to 5 xcexcm. On the other hand, if the polymeric layer is to provide a significant contribution to the mechanical integrity of the composite, a thicker polymeric layer is preferably, typically larger than 5 xcexcm. Since the time required to phase-separate increases as the combined thickness of liquid layer and polymeric layer increases it is generally desirable to keep the combined thickness as low as possible. Typically, the combined thickness would be less than 100 xcexcm or more particular less than 50 xcexcm.
The specific relative amounts of liquid and photo-polymerizable monomer in a stratified-phase-separable composition in accordance with the invention will depend on the desired ratio of liquid to polymeric layer thickness but generally will be between 1 and 99 percent by weight. Phase-separation is more easily facilitated if the relative amount of liquid or monomer ranges between 5 and 90 wt % or better between 10 and 80 wt %. The relative amount photo-polymerization dye, if added as a separate component, is determined by the desired light intensity gradient. Typically, the amount will be less than 20 wt % or even less than 10 wt % of the total weight of the stratified-phase-separable material.
To confine the liquid layer during use of the composite and/or to provide a surface on which a layer phase-separable material may be provided, a substrate may be used. Suitable substrates include glass and plastic but also metal mirror coated or silicon substrates optionally comprising integrated circuits manufactured using CMOS technology. If the composite is used for a transmissive optical application the single substrate is to be transparent. The composite in accordance with the invention may in particular combined with a flexible substrate, such as a foldable. In order to facilitate roll to roll manufacturing of the composite a wrappable substrate may be used. Suitable materials for flexible, foldable and/or wrappable single substrates include polymer films and sheets, metal foils and coated paper or laminates thereof.
In case the liquid layer is a liquid crystal layer which is to be anisotropically oriented it is convenientxe2x80x94as is well known in the artxe2x80x94to provide the substrate with an alignment layer. In particular, composite in accordance with the invention may be combined with not only a polyvinylalcohol alignment layer but also with a polyimide layer.
Combining a composite in accordance with the invention with a substrate during use and/or manufacture at least confines the liquid in directions normal to the liquid layer. In order to prevent liquid from leaking away from the composite may be packaged. Alternatively, by providing the substrate with a recess or with ridges an enclosure adapted to contain phase-separable material may be formed. After phase-separation, the polymeric layer caps the enclosure and its perimeter is attached to the side-walls of the enclosure thus obtaining a liquid tight container. The enclosure may be formed in any convenient manner for example, in the case of a plastic substrate, by injection molding. In a particular embodiment, ridges forming an enclosure may be obtained from the photo-polymerizable phase-separable material by pattern-wise photo-polymerization, eg by means of a mask having a pattern outlining the ridges to be formed.
In order to improve the mechanical integrity and stability of the stratified-phase-separated composite and/or maintain a well-defined liquid crystal layer thickness, the liquid crystal layer may comprise and/or may be partitioned by connecting (supporting) members which connect the substrate to the polymeric layer. Thus, the thickness of the connecting members exceeds the thickness of the liquid crystal layer. The connecting members may be conventional spacers which are partially embedded in the cover layer, or a relief structure pattern photo-lithographically provided on the substrate before the stratified-phase-separated composite is formed using for example a photo-resist. In a very advantageous embodiment, the connecting members are formed from pattern-wise photo-polymerizing the photo-polymerizable stratified-phase-separable coating material, eg by means of a mask. The pattern-wise photo-polymerization is conveniently performed before or simultaneous to the flood-exposure required to form the phase-separated polymeric and liquid layer.
The composite in accordance with the invention may be used for a variety of applications. In its broadest sense it may be used for any application involving a liquid. A general application if combined with a substrate is a liquid-tight packaged liquid for containing thin (0.1 xcexcm to 1 mm) films of liquid of large surface area (1 cm2 to m2). The composites in accordance with the invention allow such liquid-filled packages to be formed quickly and in an easy manner. Filling large area thin containers with liquid in the traditional manner is cumbersome. If the liquid is selected to be polymerizable, the composite in accordance with the invention may also be used for solid-state applications.
An important class of applications involves are optical and electro-optical applications in particular when the liquid is liquid crystal. In particular if the photo-polymerization is performed pattern-wise microlens arrays, gratings and structures can be manufactured.
In a preferred embodiment, the invention relates to an optical, electro-optical or display device comprising a composite in accordance with the invention The composite in accordance with the invention may comprise liquid crystal which is switchable between a first and second state, the first and second state having different optical properties such as a difference in polarization selectivity. Thus, the composite in accordance with the invention may be used in an LC display device. In principle, there is no limitation on the LC effect and device. However in a preferred embodiment an in-plane switching arrangement is used. As the composites may be manufactured in a continuous process rather than a batch process they are of particular advantage in roll-to-roll manufactured displays.
The invention also relates to a method of manufacturing a stratified-phase-separated composite in accordance with the invention. In a first embodiment, the method comprises:
providing a supporting substrate;
applying, on the substrate, a layer of photo-polymerizable stratified-phase-separable composition comprising:
a photo-polymerizable monomer;
a photo-polymerization dye; and
a liquid;
photo-polymerizing the layer of photo-polymerizable stratified-phase-separable composition to cause phase-separation into the stratified phase-separated composite comprising the liquid layer and the photo-polymeric layer.
In a broad sense, the method of this embodiment, which may also be referred as a single substrate method, provides an alternative method of forming a packaged liquid layer. The method is of particular use in case the liquid layer to be packaged is thin, say about 0.1 xcexcm to 1 mm, is of large surface area, typically form about 0.1 cm2 to about 1 m2 or more and/or has to have a uniform well-defined thickness to be kept constant during use of the packaged liquid layer. Packaging thin and large area liquid layers by filling a thin and large area container with liquid is cumbersome. The method in accordance with this embodiment is commensurate with a bottom-up process in which layers are stacked on top of the other. The method may in particular be combined with the provision of further layers by wet deposition methods such as coating and printing methods. The method may be performed in a batch process but also in a continuous process, in particular the method may be used in a roll-to-roll manufacturing process thus allowing cost-effective mass-production.
In a preferred embodiment of the single substrate method, the photo-polymerization dye selectively accumulates in the polymeric layer being formed and/or the photo-polymerizable monomer is photo-crosslinkable and/or the monomer is a (meth)acrylate.
A plurality of single substrate composites obtainable from the single method may be stacked to form a stack of single substrate stratified-phase-separated composites. Such a stack of composites may, for example, be used to obtain a multi or even full color display in which the active LC layers are stacked one on top the other to gain a factor of three in active display area. By using a single substrate to form a stacked display instead of a double substrate the distance between the active layers can be reduced to twice the thickness of the polymeric layer which may as low as 5 to 10 xcexcm. In this way parallax effects prominent in conventional stacked displays are significantly reduced.
In one embodiment, the single substrate method is repeated a number of times in succession where the single substrate stack of a previous time is used as the single substrate for a next single substrate step. Alternatively, two single substrate composites may be prepared separately and then attached to each via their polymeric layers. In this embodiment, the electrodes may be provided on both single substrates to form a single sandwich electrode arrangement or each substrate may be provided with in-plane switching electrodes to render both liquid layers (independently) switchable.
Another embodiment of the method in accordance with the invention comprises:
providing a cell adapted to contain a layer of a photo-polymerizable stratified-phase-separable composition;
filling the cell with photo-polymerizable stratified-phase-separable composition to form a layer of photo-reactive stratified-phase-separable material, the stratified-phase-separable composition comprising:
a photo-polymerizable monomer;
a photo-polymerization dye; and a liquid;
photo-polymerizing the layer of photo-polymerizable stratified-phase-separable composition to cause phase-separation into the stratified phase-separated composite comprising the liquid layer and the photo-polymeric layer.
This method, also referred to as the double substrate method, may be useful for example when very thin polymer layers are to be manufactured. Such thin polymeric layer may be desirable if the composite forms part of an LC cell in which the liquid layer of the composite is the active LC layer. In case the LC layer is to be rendered switchable by sandwiching the composite between two opposed substrates each provided with electrodes, the polymeric layer is preferably thin to reduce capacitance.
In a preferred embodiment of the double substrate method, the photo-polymerization dye selectively accumulates in the polymeric layer being formed and/or the photo-polymerizable monomer is photo-crosslinkable and/or the monomer is a (meth)acrylate.
The invention also relates to stratified-phase-separable compositions. In accordance with the invention, the composition comprises:
a photo-polymerizable monomer;
a photo-polymerization dye which, during photo-polymerization, selectively accumulates in a photo-polymeric layer being formed; and
a liquid.
In a related aspect of the invention, the composition comprises:
a photo-polymerizable monomer;
a photo-polymerization dye; and
a liquid,
wherein the photo-polymerizable monomer is an acrylate or a methacrylate monomer.
The effects and advantages associated with the compositions in accordance with the invention preferred embodiments and properties of such composites have been described hereinabove.
These and other aspects of the invention will be apparent from and elucidated with reference to the examples described hereinafter.